Methane, the principal component of natural gas, is an abundant fuel that is cheaper and cleaner burning than gasoline. Storing methane in a safe and convenient manner is critically important for facilitating the use of natural gas in automobiles. In recent years, porous metal-organic frameworks (MOFs) have emerged as promising adsorbents for methane storage. [1, 2] Thus far, several MOF compounds (PCN-14, Ni-MOF-74, UTSA-20, etc.) have been reported (by us and others) to exhibit high methane uptake at room temperature and modest pressure, surpassing the target for material-based, adsorbed methane storage set by the U.S. Department of Energy. In this talk, I am going to discuss our current mechanistic understanding of methane storage in these benchmark MOFs, based on combined experimental and computational investigations. Our recent efforts to rationally search for MOFs with even higher methane storage capacities will also be presented, and future directions will be outlined. MOFs potential for methane storage applications is enormous, but there also exist several challenges, one of which is their poor mechanical stabilities. Many MOFs suffer pore collapse, or even amorphization, under modest mechanical loadings. This makes industrial-scale processing of MOF powders rather difficult. To address this limitation, we have conducted detailed studies on the mechanical stabilities of several prototypical MOFs. [3] In this talk, I am going to discuss the origin of the low mechanical stabilities of MOFs, and propose a viable route to improve them.